title: Toward far-field vibrational spectroscopy of single molecules at room temperature.
abstract: We propose a new scheme for the extraction of chemically sensitive vibrational information from a single fluorescent molecule at room temperature. Our approach is based on a three-photon fluorescence excitation scheme, with selectivity in the production of a vibrational population of the ground state. We estimate the expected signal in perturbation theory for a standard dye molecule, compare its magnitude qualitatively to noise and various background sources, and discuss the experimental realization of this scheme.
authors.affiliation: Department of Chemistry, University of Konstanz, D-78457 Konstanz, Germany.
authors.forename: M J
authors.initials: MJ
authors.lastname: Winterhalder
authors.forename: A
authors.initials: A
authors.lastname: Zumbusch
authors.forename: M
authors.initials: M
authors.lastname: Lippitz
authors.forename: M
authors.initials: M
authors.lastname: Orrit